WO2007064557A2 - Compositions biocides solides et procedes d’utilisation de celles-ci - Google Patents

Compositions biocides solides et procedes d’utilisation de celles-ci Download PDF

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Publication number
WO2007064557A2
WO2007064557A2 PCT/US2006/045321 US2006045321W WO2007064557A2 WO 2007064557 A2 WO2007064557 A2 WO 2007064557A2 US 2006045321 W US2006045321 W US 2006045321W WO 2007064557 A2 WO2007064557 A2 WO 2007064557A2
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WO
WIPO (PCT)
Prior art keywords
solid
composition
weight
control material
desiccant
Prior art date
Application number
PCT/US2006/045321
Other languages
English (en)
Other versions
WO2007064557A3 (fr
Inventor
Huai N. Cheng
Original Assignee
Hercules Incorporated
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Hercules Incorporated filed Critical Hercules Incorporated
Priority to NZ568286A priority Critical patent/NZ568286A/en
Priority to BRPI0619191-6A priority patent/BRPI0619191A2/pt
Priority to EP06838342.1A priority patent/EP1954141B1/fr
Priority to CA2630437A priority patent/CA2630437C/fr
Priority to AU2006320788A priority patent/AU2006320788B2/en
Publication of WO2007064557A2 publication Critical patent/WO2007064557A2/fr
Priority to NO20082857A priority patent/NO20082857L/no
Publication of WO2007064557A3 publication Critical patent/WO2007064557A3/fr

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Classifications

    • A—HUMAN NECESSITIES
    • A01—AGRICULTURE; FORESTRY; ANIMAL HUSBANDRY; HUNTING; TRAPPING; FISHING
    • A01N—PRESERVATION OF BODIES OF HUMANS OR ANIMALS OR PLANTS OR PARTS THEREOF; BIOCIDES, e.g. AS DISINFECTANTS, AS PESTICIDES OR AS HERBICIDES; PEST REPELLANTS OR ATTRACTANTS; PLANT GROWTH REGULATORS
    • A01N59/00—Biocides, pest repellants or attractants, or plant growth regulators containing elements or inorganic compounds
    • A—HUMAN NECESSITIES
    • A01—AGRICULTURE; FORESTRY; ANIMAL HUSBANDRY; HUNTING; TRAPPING; FISHING
    • A01N—PRESERVATION OF BODIES OF HUMANS OR ANIMALS OR PLANTS OR PARTS THEREOF; BIOCIDES, e.g. AS DISINFECTANTS, AS PESTICIDES OR AS HERBICIDES; PEST REPELLANTS OR ATTRACTANTS; PLANT GROWTH REGULATORS
    • A01N25/00—Biocides, pest repellants or attractants, or plant growth regulators, characterised by their forms, or by their non-active ingredients or by their methods of application, e.g. seed treatment or sequential application; Substances for reducing the noxious effect of the active ingredients to organisms other than pests
    • A01N25/08—Biocides, pest repellants or attractants, or plant growth regulators, characterised by their forms, or by their non-active ingredients or by their methods of application, e.g. seed treatment or sequential application; Substances for reducing the noxious effect of the active ingredients to organisms other than pests containing solids as carriers or diluents

Definitions

  • the present invention relates to stable, pH self-adjusting, solid compositions for the preparation of biocides useful in preventing or inhibiting the growth of living organisms in liquids.
  • the present invention provides dual agent solid compositions comprising: a) a solid hypohalite; b) a solid nitrogen source; and c) a component which is either: i) a solid pH control material that has at least one secondary function as a diluent, stabilizer, anti-caking agent, binder or desiccant; or ii) a combination of a solid pH control material and a diluent, stabilizer, anti-caking agent, binder, desiccant, or combination thereof; wherein said dual agent composition forms a biocidal mixture when combined with water.
  • the present invention further provides methods of preparing a biocidal mixture comprising: a) combining a dual agent composition described herein with an amount of water suitable for producing a peak haloamine concentration of about 10 to about 10,000 ppm; or b) combining the first and second single agent solid compositions of a system described herein with an amount of water suitable for producing a peak haloamine concentration of about 10 to about 10,000 ppm.
  • the present invention further provides methods of preventing or inhibiting the growth of living organisms in a liquid comprising: a) preparing a biocidal mixture according to any of the methods described herein; and b) treating the liquid with the biocidal mixture.
  • the present invention provides, inter alia, solid dual agent compositions that, when combined with water, form biocidal mixtures useful for preventing or inhibiting growth of living organisms in liquids.
  • the components of the dual agent composition can react upon combination with water to form reactive biocidal agents including monohaloamines and/or dihaloamines (collectively "haloamines").
  • haloamines monohaloamines and/or dihaloamines
  • the solid dual agent compositions of the invention have numerous advantages over liquid and other haloamine biocidal systems including, for example, improved stability, shelf-life, portability, and general ease of use.
  • the dual agent solid compositions of the invention are further advantageously characterized by their stability and self pH-adjusting properties.
  • the solid dual agent compositions of the invention contain the following components: a) a solid hypohalite; b) a solid nitrogen source; and c) a solid pH control material.
  • the compositions can optionally further include one or more of the following solid components: d) a solid desiccant; e) a solid stabilizer; f) an anticaking agent; g) a binder; h) a disintegrant; i) a glidant; j) a solid diluent, or combination thereof.
  • Some of the components can serve multiple or overlapping functions.
  • the primary function of each component will be dictated by the name of the component.
  • the primary function of solid pH control material will be pH control of the eventual biocidal mixture.
  • the solid pH control material can also function as a diluent, stabilizer, dessicant, and/or other ingredient, but unless otherwise indicated herein, such secondary functions are optional.
  • a desiccant may also function as a diluent, stabilizer, or other ingredient. Accordingly, the desiccant' s primary function will be for protection of the composition from moisture, and any diluting or other properties will be considered secondary and therefore optional unless otherwise indicated.
  • primary function refers to the main purpose for including the ingredient in the composition and also indicates that the ingredient is present in the composition in a sufficient or effective amount to substantially carry out that function.
  • secondary function refers to a functional property of an ingredient in addition to the primary function and that the ingredient ,' is present in the composition in a sufficient or effective amount to substantially carry out both the primary and secondary functions.
  • An ingredient can have multiple secondary functions. [0011] In the case where an ingredient can potentially have multiple primary functions, it will be present in the present compositions to serve only one of those primary functions and the other functions will be considered secondary.
  • monohaloamines are formed at basic pH (e.g., greater than about pH 8); dihaloamines are formed from monohaloamines at acidic pH (e.g., at about pH 3-5); and trihaloamines are formed at very acidic pH (e.g., at about pH ⁇ 3).
  • pH can be controlled by the amount and type of solid pH control material used in the composition, thereby allowing regulation of the type as well as amount of haloamine generated in the biocidal mixture.
  • the pH control material also ultimately eliminates or reduces the need for subsequent pH adjustments or titrations of the biocidal mixture. This characteristic is one of the numerous advantages of the present invention.
  • the optional desiccant, diluent, stabilizer, and other components of the compositions of the invention can influence stability and other properties of the solid compositions.
  • the solid hypohalite component can be a solid hypohalite salt including an alkali metal or alkaline earth metal hypohalite salt.
  • Suitable solid hypohalites include magnesium, lithium, or calcium salts of hypochlorite, hypobromite, or hypoiodite.
  • Example solid hypohalites include calcium hypochlorite and lithium hypochlorite.
  • the solid hypohalite is calcium hypochlorite.
  • the pH control material can be any solid substance capable of maintaining or achieving a desired pH when the composition is mixed with water in order to obtain the desired compounds (e.g., monochloramine and/or dichloramine).
  • the pH control material is an inorganic salt (e.g., an alkali metal or alkaline earth metal salt) of a hydroxide (e.g., sodium hydroxide), carbonate (e.g., sodium carbonate, potassium carbonate, and the like), acetate (e.g., sodium acetate), phosphate, or other substance capable of keeping a solution at basic pH.
  • a hydroxide e.g., sodium hydroxide
  • carbonate e.g., sodium carbonate, potassium carbonate, and the like
  • acetate e.g., sodium acetate
  • phosphate or other substance capable of keeping a solution at basic pH.
  • the solid pH control material maintains the biocidal mixture at a pH of about 8 to about 13, about 9 to about 12, about 10, or about 11.
  • the pH control material is sodium hydroxide or sodium carbonate.
  • the pH control material can include a substance capable of keeping a solution at acidic pH.
  • the pH control material can be an inorganic salt of hydrogen phthalate or monobasic sodium phosphate.
  • the solid pH control material maintains the biocidal mixture at a pH of about 3 to about 6, about 3 to about 5, or about 4. It is sometimes desirable that the pH control material has relatively poor water solubility compared to the active agents. For example, lower solubility can delay acidification thereby allowing monohaloamines to be formed first at higher pH. The monohaloamines can then serve as precursors to the dihaloamines which are subsequently formed when the pH control material eventually dissolves and the solution reaches the desired acidic pH.
  • pH control materials can include inorganic salts of the following substances: borate, phosphate, propionate, butyrate, or mixtures of these and the like.
  • the solid pH control material has a secondary function as a diluent, such as when there is sufficient quantity of the solid pH control material to effectively dilute and disperse the actives (e.g., the solid nitrogen source and solid hypohalite) such that interaction between the solid actives is minimized thereby facilitating composition stability and extending shelf-life.
  • Solid pH control materials having a secondary function as a diluent include, for example, substances containing salts of carbonate, such as sodium carbonate or potassium carbonate, or inorganic salts of hydrogen phthalate.
  • the solid pH control material has a secondary function as a desiccant, meaning that it preferentially absorbs and sequesters water vapor from the ambient surroundings serving to protect the moisture sensitive components (e.g., the actives) of the compositions of the invention and benefit stability.
  • Example solid pH control materials that have a secondary function as a desiccant include, for example, substances containing salts of carbonate, such as potassium carbonate or sodium carbonate.
  • the solid pH control material can have secondary functions of both diluent and desiccant.
  • the dual agent compositions of the invention can further include a diluent.
  • the diluent can be any solid substance serving to disperse and dilute one or more of the reactive components (actives) of the solid composition to effectively minimize their interaction in solid form. Diluents are typically inert toward the actives. A diluent may also have a secondary function as a binder, stabilizer, anticaking agent, or other function. Some diluents may also function as desiccants. In some embodiments, the diluent does not have a secondary function as a pH control material, hi some embodiments, the diluent does not have a secondary function as a stabilizer.
  • Suitable diluents include inorganic salts (e.g., NaCl, KCl, sodium carbonate, potassium carbonate, calcium sulfates, calcium phosphates, metal aluminosilicates, etc.) as well as powdered cellulose, PCC, and microcrystalline cellulose (e.g., Avicel), and the like.
  • inorganic salts e.g., NaCl, KCl, sodium carbonate, potassium carbonate, calcium sulfates, calcium phosphates, metal aluminosilicates, etc.
  • powdered cellulose PCC
  • microcrystalline cellulose e.g., Avicel
  • a desiccant can be any solid hygroscopic material that preferentially absorbs and sequesters water vapor from the ambient surroundings, serving to protect the moisture sensitive components of the compositions.
  • Suitable solid desiccants include activated alumina, silica gel, calcium chloride, zinc chloride, calcium sulfate (e.g., anhydrous calcium sulfate), calcium oxide, potassium carbonate, montmorillonite clay, and the like.
  • the desiccant contains anhydrous calcium sulfate (e.g., Drierite® from W. A. Hammond Company, Xenia, Ohio) or potassium carbonate.
  • Other suitable desiccants are provided in, for example, A. P.
  • the desiccant does not have a secondary function as a solid pH control material.
  • Example desiccants that do not necessarily have a secondary function as solid pH control materials include alumina, silica gel, calcium chloride, zinc chloride, calcium sulfate (e.g., anhydrous calcium sulfate), calcium oxide, montmorillonite clay, and the like.
  • the dual agent compositions of the invention can further contain other solid additives such as stabilizers, anticaking agents, binders, disintegrants, and glidants.
  • a suitable stabilizer can be any solid substance that works to extend the shelf- life of a solid dual agent composition of the invention.
  • the stabilizer is a substance that does not have a secondary function as a pH control material and/or a desiccant.
  • Example stabilizers include inorganic salts such as alkali and alkaline earth metal salts of halides and sulfate such as sodium chloride, sodium sulfate, mixtures thereof and the like.
  • a suitable anticaking agent serves to help keep powders free flowing and to facilitate the ready dissolution of a powder in water.
  • Example anticaking agents include sodium chloride, sodium carbonate, potassium carbonate, dibasic calcium phosphate (anhydrous), silicon dioxide (silica), calcium silicate, precipitated calcium carbonate (PCC), and the like.
  • the dual agent compositions of the invention can further include a binder.
  • the dual agent compositions of the invention can further include a disintegrant.
  • Suitable disintegrants can include, for example, sodium chloride, sodium sulfate, ammonium chloride, ammonium sulfate, microcrystalline cellulose, and the like.
  • the dual agent compositions of the invention can further include a glidant.
  • Suitable glidants include, for example, magnesium stearate, calcium stearate, talc, colloidal silicas (e.g., Aerosil 200), carnauba wax, hydrogenated vegetable oils, mineral oil, polyethylene glycols, and the like.
  • the dual agent compositions of the invention can contain various ratios and amounts of the components such that the biocidal monohaloamine and/or dihaloamine agent is generated upon dissolution of the composition in water.
  • the amount of solid nitrogen source individually present in the dual agent compositions of the invention can be, for example, about 1 to about 23, about 2 to about 15, about 5 to about 10, or about 8 wt%.
  • the amount of solid hypohalite individually present in the dual agent compositions of the invention can be, for example, about 1 to about 27, about 2 to about 20, about 5 to about 15, or about 12 wt%.
  • the solid hypohalite and solid nitrogen source can be considered the active ingredients of the dual agent compositions of the invention and these two ingredients together are referred to herein as "active agents" or "actives.”
  • the dual agent compositions of the invention can be prepared such that the actives make up about 50% or less of the total weight of the composition.
  • actives can make up about 5 to about 50%, about 5 to about 30%, about 10 to about 30%, about 15 to about 25%, or about 20% of the total weight of the composition.
  • Compositions containing 1 to about 5% of the actives are also contemplated by the invention.
  • compositions of the invention can contain about 0.5 to about 25, about 1 to about 15, or about 1 to about 10 wt% of pH control material which contains a relatively strong base (e.g., hydroxide). In other embodiments, compositions of the invention can contain about 20 to about 90, about 60 to about 90, or about 80 wt% of pH control material containing a relatively weak base (e.g., carbonate).
  • a relatively strong base e.g., hydroxide
  • compositions of the invention can contain about 20 to about 90, about 60 to about 90, or about 80 wt% of pH control material containing a relatively weak base (e.g., carbonate).
  • pH control material can be present in compositions of the invention in amounts of about 50 to about 95, about 70 to about 90, about 75 to about 85; about 20 to about 80, about 20 to about 75, about 20 to about 30; about 55 to about 67, about 40 to about 95, about 40 to about 80, about 40 to about 60, about 50 to about 70, about 30 to about 90; about 1 to about 5, about 1 to about 3, about 80, about 60, about 25, or about 2.5 wt%.
  • the dual agent compositions contain a further (i.e., a second) pH control material. Suitable amounts include 0 to about 55, 0 to about 40, or about
  • dual agent compositions containing a desiccant any appropriate amount can be used. In some embodiments, dual agent compositions contain 15 to about 80, about
  • the desiccant can also function as a pH control material.
  • An example dual function desiccant and pH control material is potassium carbonate.
  • compositions containing other solid additives the appropriate amount will depend on the properties and amounts of the other components.
  • a strongly reactive substance such as a strong base (e.g., hydroxide)
  • greater amounts of the solid additives such as stabilizer and/or diluent can be employed.
  • the pH control material can have the same diluting affect as a diluent, so less (or no) diluent or other additives may be needed.
  • the dual agent compositions of the invention can contain about 0 to about 55, about 0 to about 40, about 1 to about 83, about 10 to about
  • dual agent compositions containing a stabilizer the appropriate amount will depend on the properties and the amounts of the other components. In some embodiments, dual agent compositions contain about 40 to about 75 wt %, about 50 to about
  • Anticaking agents can be present in the dual agent compositions of the invention in amounts of about 0.1 to about 50, about 0.1 to about 10, and about 0.1 to about 5 wt%.
  • compositions of the invention can be individually present in the dual agent compositions of the invention, such as dual agent compositions suitable for preparing tablets or bars, in an amount of about 0.2 to about 5 wt%, about 0.5 to about 2 wt%, about 0.5 to about 1 wt%, or about 1 wt%.
  • Certain example dual agent compositions according to the present invention consist essentially of (e.g.,. greater than about 95% of total weight): a) a solid hypohalite; b) an ammonium salt; and ,- c) a solid pH control material.
  • the solid pH control material can have a secondary function as a diluent, stabilizer, anti-caking agent, binder, or desiccant substantially obviating the need for these ingredients as separate components of the composition.
  • the solid pH control material is an inorganic salt of carbonate such as sodium carbonate or potassium carbonate.
  • Further related example dual agent compositions Al, A2, A3, and A4 are provided in Table A below (percentages are provided as wt%). For each of the example dual agent compositions, the N/X ratio is about 1.5: 1 to about 0.8:1.
  • An example dual agent composition that employs a desiccant contains: a) about 5 to about 30 % by weight of said solid hypohalite and said solid nitrogen source, together; b) about 20 to about 80 % by weight of a solid pH control material that has at least one secondary function (such as a diluent); and c) about 15 to about 75 % by weight of desiccant.
  • potassium carbonate has the remarkable advantage of serving five functions at once: diluent, anti-caking, pH control, stabilizer, and desiccant.
  • Example 5 Dual Agent Powder Compositions Containing a Stabilizer
  • Two tables are shown for example compositions containing a stabilizer.
  • a further pH control system that can be used for generating DCA is monobasic sodium phosphate (Table 8-2).
  • the overall Hach value is lower, but the formulation is stable.

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  • Life Sciences & Earth Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Dentistry (AREA)
  • Pest Control & Pesticides (AREA)
  • Plant Pathology (AREA)
  • Engineering & Computer Science (AREA)
  • Agronomy & Crop Science (AREA)
  • Wood Science & Technology (AREA)
  • Zoology (AREA)
  • Environmental Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Chemical & Material Sciences (AREA)
  • Toxicology (AREA)
  • Agricultural Chemicals And Associated Chemicals (AREA)
  • Medicinal Preparation (AREA)

Abstract

La présente invention concerne des compositions stables, solides, à pH auto-régulable, destinées à la préparation d'un biocide utile dans la prévention ou l’inhibition de la croissance d’organismes vivants dans des liquides.
PCT/US2006/045321 2005-11-30 2006-11-22 Compositions biocides solides et procedes d’utilisation de celles-ci WO2007064557A2 (fr)

Priority Applications (6)

Application Number Priority Date Filing Date Title
NZ568286A NZ568286A (en) 2005-11-30 2006-11-22 Solid biocidal compositions comprising a hypohalite and a nitrogen source
BRPI0619191-6A BRPI0619191A2 (pt) 2005-11-30 2006-11-22 composições biocidas sólidas e métodos de uso mesmas
EP06838342.1A EP1954141B1 (fr) 2005-11-30 2006-11-22 Compositions biocides solides et procedes d'utilisation de celles-ci
CA2630437A CA2630437C (fr) 2005-11-30 2006-11-22 Compositions biocides solides et procedes d'utilisation de celles-ci
AU2006320788A AU2006320788B2 (en) 2005-11-30 2006-11-22 Solid biocidal compositions and methods of using the same
NO20082857A NO20082857L (no) 2005-11-30 2008-06-23 Faste biocidale sammensetninger og anvendelser derav

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US11/289,990 US20070123423A1 (en) 2005-11-30 2005-11-30 Solid biocidal compositions and methods of using the same
US11/289,990 2005-11-30

Publications (2)

Publication Number Publication Date
WO2007064557A2 true WO2007064557A2 (fr) 2007-06-07
WO2007064557A3 WO2007064557A3 (fr) 2009-03-05

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PCT/US2006/045321 WO2007064557A2 (fr) 2005-11-30 2006-11-22 Compositions biocides solides et procedes d’utilisation de celles-ci

Country Status (11)

Country Link
US (2) US20070123423A1 (fr)
EP (1) EP1954141B1 (fr)
KR (1) KR20080072016A (fr)
CN (1) CN101494986A (fr)
AU (1) AU2006320788B2 (fr)
BR (1) BRPI0619191A2 (fr)
CA (1) CA2630437C (fr)
NO (1) NO20082857L (fr)
NZ (1) NZ568286A (fr)
WO (1) WO2007064557A2 (fr)
ZA (1) ZA200805711B (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP3110459A4 (fr) * 2014-02-27 2017-08-16 Bromine Compounds Ltd. Composition biocide, préparation et procédés d'utilisation associés

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US9388044B2 (en) 2006-12-29 2016-07-12 Nalco Company Methods for the on-site production of chloramine and uses thereof
PT3357870T (pt) 2013-02-07 2022-08-30 A Y Lab Ltd Método para controlar a produção de um biocida
CA2932704C (fr) * 2013-12-05 2022-06-28 Buckman Laboratories International, Inc. Procedes de regulation microbiologique dans le traitement d'une matiere contenant du sucre de betterave et d'autres sucres
JP6722569B2 (ja) * 2016-11-18 2020-07-15 花王株式会社 モノハロゲノアミンの製造方法
JP6935301B2 (ja) * 2016-11-18 2021-09-15 花王株式会社 モノハロゲノアミン製造用被覆粒子群
JP6759068B2 (ja) * 2016-11-18 2020-09-23 花王株式会社 モノハロゲノアミン製造用固体組成物
JP6875111B2 (ja) * 2016-12-01 2021-05-19 花王株式会社 モノハロゲノアミン製造用組成物
JP2021166949A (ja) * 2020-04-09 2021-10-21 株式会社ユーディー 水蒸気吸放出材料、それを用いる除湿剤および除湿方法

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GB1126108A (en) * 1965-07-02 1968-09-05 Olin Mathieson Deoderizing tablet and method
EP0005286A1 (fr) * 1978-04-18 1979-11-14 THE PROCTER & GAMBLE COMPANY Composition désinfectante solide et compacte contenant un mélange d'hypochlorite de lithium et d'hypochlorite de calcium
EP1029912A1 (fr) * 1999-02-16 2000-08-23 The Procter & Gamble Company Compositions de blanchiment composées d'un oligocarboxylate et d'un agent complexant
EP1293482A1 (fr) * 1991-06-03 2003-03-19 Bromine Compounds Ltd. Procédé pour la désinfection de l'eau
EP1557088A1 (fr) * 2004-01-20 2005-07-27 A-Dec, Inc. Traitement à effet prolongé de l'eau utilisée dans les équipements dentaires

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GB1126108A (en) * 1965-07-02 1968-09-05 Olin Mathieson Deoderizing tablet and method
EP0005286A1 (fr) * 1978-04-18 1979-11-14 THE PROCTER & GAMBLE COMPANY Composition désinfectante solide et compacte contenant un mélange d'hypochlorite de lithium et d'hypochlorite de calcium
EP1293482A1 (fr) * 1991-06-03 2003-03-19 Bromine Compounds Ltd. Procédé pour la désinfection de l'eau
EP1029912A1 (fr) * 1999-02-16 2000-08-23 The Procter & Gamble Company Compositions de blanchiment composées d'un oligocarboxylate et d'un agent complexant
EP1557088A1 (fr) * 2004-01-20 2005-07-27 A-Dec, Inc. Traitement à effet prolongé de l'eau utilisée dans les équipements dentaires

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP3110459A4 (fr) * 2014-02-27 2017-08-16 Bromine Compounds Ltd. Composition biocide, préparation et procédés d'utilisation associés

Also Published As

Publication number Publication date
NO20082857L (no) 2008-08-15
BRPI0619191A2 (pt) 2011-09-13
US20070123423A1 (en) 2007-05-31
US20140080707A1 (en) 2014-03-20
EP1954141A2 (fr) 2008-08-13
CN101494986A (zh) 2009-07-29
AU2006320788A1 (en) 2007-06-07
KR20080072016A (ko) 2008-08-05
NZ568286A (en) 2011-08-26
CA2630437C (fr) 2013-06-25
ZA200805711B (en) 2009-11-25
WO2007064557A3 (fr) 2009-03-05
AU2006320788B2 (en) 2012-07-26
EP1954141B1 (fr) 2016-03-09
CA2630437A1 (fr) 2007-06-07

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